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There are many vibration energy in nature, vibration energy harvesting is an attractive technique for low-power devices. In this paper, a new vibration energy harvesting by carbon nanotube network(NTN)/polydimethylsiloxane(PDMS) composite was investigated. The composite of NTN embedded in PDMS matrix has been fabricated by using filtration, standard integrated circuits processes and transfer process. The NTN/PDMS composite can be used to harvest energy from vibrating structures. The energy harvesting device is not only single resonance frequency based, but also used to a frequency range of vibration energy. The NTN/PDMS composite provides a new approach to harvest vibration energy.